Journal Article•
Self-organization of CdSe nanocrystallites into three-dimensional quantum dot superlattices
01 Jan 2005-SPIE milestone series (Society of Photo-Optical Instrumentation Engineers)-Vol. 180, pp 64-67
TL;DR: In this paper, the self-organization of CdSe nanocrystallites into three-dimensional semiconductor quantum dot superiattices (colloidal crystals) is demonstrated.
Abstract: The self-organization of CdSe nanocrystallites into three-dimensional semiconductor quantum dot superiattices (colloidal crystals) is demonstrated. The size and spacing of the dots within the superlattice are controlled with near atomic precision. This control is a result of synthetic advances that provide CdSe nanocrystallites that are monodisperse within the limit of atomic roughness. The methodology is not limited to semiconductor quantum dots but provides general procedures for the preparation and characterization of ordered structures of nanocrystallites from a variety of materials.
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01 Mar 1998
TL;DR: The quantum-confined Stark effect in single cadmium selenide (CdSe) nanocrystallite quantum dots was studied, suggesting the potential use of these dots in electro-optic modulation devices.
Abstract: The quantum-confined Stark effect in single cadmium selenide (CdSe) nanocrystallite quantum dots was studied. The electric field dependence of the single-dot spectrum is characterized by a highly polarizable excited state (∼10 5 cubic angstroms, compared to typical molecular values of order 10 to 100 cubic angstroms), in the presence of randomly oriented local electric fields that change over time. These local fields result in spontaneous spectral diffusion and contribute to ensemble inhomogeneous broadening. Stark shifts of the lowest excited state more than two orders of magnitude larger than the linewidth were observed, suggesting the potential use of these dots in electro-optic modulation devices.
696 citations
Journal Article•
TL;DR: In this article, the solid Cd 10 S 4 (SC 6 H 5 ) 12 from a solution of pyridine and N,N-di-methytformamide (DMF) results in the formation of the cluster Cd 32 S 1 4(SC 6H 5 ) 36 -DMF 4 as pale yellow cubes.
Abstract: Recrystallization of the solid Cd 10 S 4 (SC 6 H 5 ) 12 from a solution of pyridine and N,N-di-methytformamide (DMF) results in the formation of the cluster Cd 32 S 1 4 (SC 6 H 5 ) 36 -DMF 4 as pale yellow cubes. The structure consists of an 82-atom CdS core that is a roughly spherical piece of the cubic sphalerite lattice -12 angstroms in diameter. The four corners of the lattice are capped by hexagonal wurtzite-like CdS units, which results in an overall tetrahedral cluster ∼ 15 angstroms in diameter. This cluster dissolves intact in tetrahydrofuran where its absorption spectrum reveals a sharp peak at 358 nanometers at room temperature and its emission spectra show a strong broad band at 500 nanometers.
318 citations
Dissertation•
01 Jan 2016
TL;DR: In this paper, the authors used Förster theory to understand the photoluminescence and vibrational characteristics of QDs, including spectrally-resolved time-correlated single photon counting measurements to understand QD photon lifetime as a function of emission wavelength and low-frequency Raman spectroscopy to measure acoustic phonons in nanocrystal solids.
Abstract: Semiconductor nanocrystals, also known as quantum dots (QDs) have been used in solid state light emission applications ranging from fluorescent downconverters to LEDs and lasers, as well as energy generation devices such as solar photovoltaics and thermoelectrics. In order to realize these myriad applications, the fundamental physics of both electronic and vibrational energy transfer must be understood to engineer better device performance. This thesis begins with a general introduction to the physics and chemistry of QDs as well as an introduction to lattice vibrations, including a proposed model for understanding thermal conductivity in solid state QD-based devices. It continues with a discussion of the methods used to understand the photoluminescence and vibrational characteristics of QDs, including spectrallyresolved time-correlated single photon counting measurements to understand QD photoluminescence lifetime as a function of emission wavelength, and low-frequency Raman spectroscopy to measure acoustic phonons in nanocrystal solids. These two chapters serve as an introduction to the ideas and methods used throughout the thesis. In Chapter 3, Förster theory is used in conduction with spectrallyand temporallyresolved photoluminescence spectroscopy to understand the rates of excitonic energy transfer in CdSe/CdZnS core/shell QDs through a calculation of the effective dipoledipole coupling distance known as the Förster radius. This work demonstrated energy transfer rates between donor and acceptor QDs between 10-100 times faster than the predictions based on standard applications of Förster theory, corresponding to an effective Förster radius of 8-9 nm in close packed QD films. Several possible effects, including an enhanced absorption cross section, ordered dipole orientations, or dipolemultipole coupling, can explain the observed difference between our measurements and the Förster theory predictions, demonstrating that several standard assumptions commonly used for calculating QD resonant energy transfer rates must be carefully considered when the QDs are in a thin-film geometry. Chapters 4-5 involve the use of low-frequency Raman spectroscopy to probe acoustic phonons in QDs. These low-frequency acoustic vibrations affect the
9 citations
01 Jan 2019
TL;DR: In this article, the authors discuss the importance of the role of the human voice in the decision process and propose a method to improve the quality of the decision making process of the board.
Abstract: . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . x CHAPTER
8 citations
References
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TL;DR: In this article, the authors focus on the properties of quantum dots and their ability to join the dots into complex assemblies creates many opportunities for scientific discovery, such as the ability of joining the dots to complex assemblies.
Abstract: Current research into semiconductor clusters is focused on the properties of quantum dots-fragments of semiconductor consisting of hundreds to many thousands of atoms-with the bulk bonding geometry and with surface states eliminated by enclosure in a material that has a larger band gap. Quantum dots exhibit strongly size-dependent optical and electrical properties. The ability to join the dots into complex assemblies creates many opportunities for scientific discovery.
10,737 citations
TL;DR: In this paper, a simple route to the production of high-quality CdE (E=S, Se, Te) semiconductor nanocrystallites is presented, based on pyrolysis of organometallic reagents by injection into a hot coordinating solvent.
Abstract: A simple route to the production of high-quality CdE (E=S, Se, Te) semiconductor nanocrystallites is presented. Crystallites from ∼12 A to ∼115 A in diameter with consistent crystal structure, surface derivatization, and a high degree of monodispersity are prepared in a single reaction. The synthesis is based on the pyrolysis of organometallic reagents by injection into a hot coordinating solvent. This provides temporally discrete nucleation and permits controlled growth of macroscopic quantities of nanocrystallites. Size selective precipitation of crystallites from Portions of the growth solution isolates samples with narrow size distributions (<5% rms in diameter). High sample quality results in sharp absorption features and strong «band-edge» emission which is tunable with particle size and choice of material
8,374 citations
TL;DR: Highly luminescent semiconductor quantum dots (zinc sulfide-capped cadmium selenide) have been covalently coupled to biomolecules for use in ultrasensitive biological detection and these nanometer-sized conjugates are water-soluble and biocompatible.
Abstract: Highly luminescent semiconductor quantum dots (zinc sulfide-capped cadmium selenide) have been covalently coupled to biomolecules for use in ultrasensitive biological detection. In comparison with organic dyes such as rhodamine, this class of luminescent labels is 20 times as bright, 100 times as stable against photobleaching, and one-third as wide in spectral linewidth. These nanometer-sized conjugates are water-soluble and biocompatible. Quantum dots that were labeled with the protein transferrin underwent receptor-mediated endocytosis in cultured HeLa cells, and those dots that were labeled with immunomolecules recognized specific antibodies or antigens.
7,393 citations
IBM1
TL;DR: Thermal annealing converts the internal particle structure from a chemically disordered face- centered cubic phase to the chemically ordered face-centered tetragonal phase and transforms the nanoparticle superlattices into ferromagnetic nanocrystal assemblies that can support high-density magnetization reversal transitions.
Abstract: Synthesis of monodisperse iron-platinum (FePt) nanoparticles by reduction of platinum acetylacetonate and decomposition of iron pentacarbonyl in the presence of oleic acid and oleyl amine stabilizers is reported. The FePt particle composition is readily controlled, and the size is tunable from 3- to 10-nanometer diameter with a standard deviation of less than 5%. These nanoparticles self-assemble into three-dimensional superlattices. Thermal annealing converts the internal particle structure from a chemically disordered face-centered cubic phase to the chemically ordered face-centered tetragonal phase and transforms the nanoparticle superlattices into ferromagnetic nanocrystal assemblies. These assemblies are chemically and mechanically robust and can support high-density magnetization reversal transitions.
5,568 citations
TL;DR: In this article, solution phase syntheses and size-selective separation methods to prepare semiconductor and metal nanocrystals, tunable in size from ∼1 to 20 nm and monodisperse to ≤ 5%, are presented.
Abstract: ▪ Abstract Solution phase syntheses and size-selective separation methods to prepare semiconductor and metal nanocrystals, tunable in size from ∼1 to 20 nm and monodisperse to ≤5%, are presented. Preparation of monodisperse samples enables systematic characterization of the structural, electronic, and optical properties of materials as they evolve from molecular to bulk in the nanometer size range. Sample uniformity makes it possible to manipulate nanocrystals into close-packed, glassy, and ordered nanocrystal assemblies (superlattices, colloidal crystals, supercrystals). Rigorous structural characterization is critical to understanding the electronic and optical properties of both nanocrystals and their assemblies. At inter-particle separations 5–100 A, dipole-dipole interactions lead to energy transfer between neighboring nanocrystals, and electronic tunneling between proximal nanocrystals gives rise to dark and photoconductivity. At separations <5 A, exchange interactions cause otherwise insulating ass...
4,116 citations